Ag/LaCoO3 perovskite catalysts for soot combustion were prepared by the impregnation method.The structure and physicochemical properties of the catalysts were characterized using X-ray diffraction,N2 adsorption-desorp...Ag/LaCoO3 perovskite catalysts for soot combustion were prepared by the impregnation method.The structure and physicochemical properties of the catalysts were characterized using X-ray diffraction,N2 adsorption-desorption,H2 temperature-programmed reduction,soot temperatureprogrammed reduction,and X-ray photoelectron spectroscopy.The catalytic activity of the catalysts for soot oxidation was tested by temperature-programmed oxidation in air and in a NOx atmosphere.Metallic Ag particles were the main Ag species.Part of the Ag migrated from the surface to the lattice of the LaCoO3 perovskite,to form La（1-x）AgxCoO3.This increased the amount of oxygen vacancies in the perovskite structure during thermal treatment.Compared with unmodified LaCoO3,the maximum soot oxidation rate temperature（Tp） decreased by 50-70 ℃ in air when LaCoO3 was partially modified by Ag,depending on the thermal treatment temperature.The Tp of the Ag/LaCoO3catalyst calcined at 400℃ in a NOx atmosphere decreased to about 140℃,compared with that of LaCoO3.Ag particles and oxygen vacancies in the catalysts contributed to their high catalytic activity for soot oxidation.The stable catalytic activity of the Ag/LaCoO3 catalyst calcined at 700℃ in a NOx atmosphere was related to its stable structure.展开更多
Combinations of graphene(Gr)and carbon black(C)were employed as binary carbon supports to fabricate Pd‐based electrocatalysts via one‐pot co‐reduction with Pd2+.The electrocatalytic performance of the resulting Pd...Combinations of graphene(Gr)and carbon black(C)were employed as binary carbon supports to fabricate Pd‐based electrocatalysts via one‐pot co‐reduction with Pd2+.The electrocatalytic performance of the resulting Pd/Gr‐C catalysts during the electrooxidation of formic acid was assessed.A Pd/Gr0.3C0.7(Gr oxide:C=3:7,based on the precursor mass ratio)electrocatalyst exhibited better catalytic performance than both Pd/C and Pd/Gr catalysts.The current density generated by the Pd/Gr0.3C0.7catalyst was as high as102.14mA mgPd?1,a value that is approximately3times that obtained from the Pd/C(34.40mA mgPd?1)and2.6times that of the Pd/Gr material(38.50mA mgPd?1).The anodic peak potential of the Pd/Gr0.3C0.7was120mV more negative than that of the Pd/C and70mV more negative than that of the Pd/Gr.Scanning electron microscopy images indicated that the spherical C particles accumulated on the wrinkled graphene surfaces to form C cluster/Gr hybrids having three‐dimensional nanostructures.X‐ray photoelectron spectroscopy data confirmed the interaction between the Pd metal and the binary Gr‐C support.The Pd/Gr0.3C0.7also exhibited high stability,and so is a promising candidate for the fabrication of anodes for direct formic acid fuel cells.This work demonstrates a simple and cost‐effective method for improving the performance of Pd‐based electrocatalysts,which should have potential industrial applications.展开更多
基金supported by the National Basic Research Program of China (973 Program,2009CB220010)the National Natural Science Foundation of China (20603016)+1 种基金the Scientific Research Fund of Liaoning Provincial Education Department (L2010222)Liaoning Provincial Science&Technology Project of China (20071074)~~
文摘Ag/LaCoO3 perovskite catalysts for soot combustion were prepared by the impregnation method.The structure and physicochemical properties of the catalysts were characterized using X-ray diffraction,N2 adsorption-desorption,H2 temperature-programmed reduction,soot temperatureprogrammed reduction,and X-ray photoelectron spectroscopy.The catalytic activity of the catalysts for soot oxidation was tested by temperature-programmed oxidation in air and in a NOx atmosphere.Metallic Ag particles were the main Ag species.Part of the Ag migrated from the surface to the lattice of the LaCoO3 perovskite,to form La（1-x）AgxCoO3.This increased the amount of oxygen vacancies in the perovskite structure during thermal treatment.Compared with unmodified LaCoO3,the maximum soot oxidation rate temperature（Tp） decreased by 50-70 ℃ in air when LaCoO3 was partially modified by Ag,depending on the thermal treatment temperature.The Tp of the Ag/LaCoO3catalyst calcined at 400℃ in a NOx atmosphere decreased to about 140℃,compared with that of LaCoO3.Ag particles and oxygen vacancies in the catalysts contributed to their high catalytic activity for soot oxidation.The stable catalytic activity of the Ag/LaCoO3 catalyst calcined at 700℃ in a NOx atmosphere was related to its stable structure.
基金supported by the Natural Science Foundation of Shandong Province(ZR2016BM31)the Science and Technology Foundation of Jinan City(201311035)~~
文摘Combinations of graphene(Gr)and carbon black(C)were employed as binary carbon supports to fabricate Pd‐based electrocatalysts via one‐pot co‐reduction with Pd2+.The electrocatalytic performance of the resulting Pd/Gr‐C catalysts during the electrooxidation of formic acid was assessed.A Pd/Gr0.3C0.7(Gr oxide:C=3:7,based on the precursor mass ratio)electrocatalyst exhibited better catalytic performance than both Pd/C and Pd/Gr catalysts.The current density generated by the Pd/Gr0.3C0.7catalyst was as high as102.14mA mgPd?1,a value that is approximately3times that obtained from the Pd/C(34.40mA mgPd?1)and2.6times that of the Pd/Gr material(38.50mA mgPd?1).The anodic peak potential of the Pd/Gr0.3C0.7was120mV more negative than that of the Pd/C and70mV more negative than that of the Pd/Gr.Scanning electron microscopy images indicated that the spherical C particles accumulated on the wrinkled graphene surfaces to form C cluster/Gr hybrids having three‐dimensional nanostructures.X‐ray photoelectron spectroscopy data confirmed the interaction between the Pd metal and the binary Gr‐C support.The Pd/Gr0.3C0.7also exhibited high stability,and so is a promising candidate for the fabrication of anodes for direct formic acid fuel cells.This work demonstrates a simple and cost‐effective method for improving the performance of Pd‐based electrocatalysts,which should have potential industrial applications.
